Wang Dongsheng, Fan Mingyue, He Tingyu, Zeng Fanming, Hu Xiaoli, Li Chun, Su Zhongmin
School of Materials Science and Engineering, Changchun University of Science and Technology, Changchun, 130022, P. R. China.
Jilin Provincial Science and Technology Innovation Center of Optical Materials and Chemistry, Changchun University of Science and Technology, Changchun, 130022, P. R. China.
Chemistry. 2021 Aug 5;27(44):11468-11476. doi: 10.1002/chem.202101560. Epub 2021 Jun 8.
The reasonable design of the precursor of a carbon-based nanocatalyst is an important pathway to improve catalytic performance. In this study, a simple solvothermal method was used to synthesize [Cu(TPT)(2,5-tdc)] ⋅ 2H O (Cu-MOF), which contains N and S atoms, in one step. Further in-situ carbonization of the Cu-MOF as the precursor was used to synthesize Cu/Cu S-embedded N,S-doped porous carbon (Cu/Cu S/NSC) composites. The catalytic activities of the prepared Cu/Cu S/NSC were investigated through catalytic reduction of 4-nitrophenol (4-NP) to 4-aminophenol (4-AP). The results show that the designed Cu/Cu S/NSC has exceptional catalytic activity and recycling stability, with a reaction rate constant of 0.0256 s , and the conversion rate still exceeds 90 % after 15 cycles. Meanwhile, the efficient catalytic reduction of dyes (CR, MO, MB and RhB) confirmed its versatility. Finally, the active sites of the Cu/Cu S/NSC catalysts were analyzed, and a possible multicomponent synergistic catalytic mechanism was proposed.
碳基纳米催化剂前驱体的合理设计是提高催化性能的重要途径。在本研究中,采用简单的溶剂热法一步合成了含N和S原子的[Cu(TPT)(2,5-tdc)]⋅2H₂O(Cu-MOF)。以Cu-MOF为前驱体进一步原位碳化,合成了Cu/Cu₂S嵌入的N、S掺杂多孔碳(Cu/Cu₂S/NSC)复合材料。通过催化4-硝基苯酚(4-NP)还原为4-氨基苯酚(4-AP)研究了所制备的Cu/Cu₂S/NSC的催化活性。结果表明,所设计的Cu/Cu₂S/NSC具有优异的催化活性和循环稳定性,反应速率常数为0.0256 s⁻¹,15次循环后转化率仍超过90%。同时,对染料(CR、MO、MB和RhB)的高效催化还原证实了其通用性。最后,分析了Cu/Cu₂S/NSC催化剂的活性位点,并提出了可能的多组分协同催化机理。